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A Record-High Cryogenic Magnetocaloric Effect Discovered in EuCl<sub>2</sub> Compound

Bingjie Wang, Xin‐Yang Liu, Fengxia Hu, Jian-Tao Wang, Jian-Tao Wang, Junsen Xiang, Peijie Sun, Jing Wang, Jing Wang, Jirong Sun, Tongyun Zhao, Zhaojun Mo, Jun Shen, Yunzhong Chen, Q. Huang, Baogen Shen

2024Journal of the American Chemical Society36 citationsDOI

Abstract

Adiabatic demagnetization refrigeration (ADR) based on the magnetocaloric effect (MCE) is a promising technique to achieve cryogenic temperature. However, magnetic entropy change (Δ S M ), the driving force of ADR, remains far below theoretical −Δ S M = nR ln(2 J + 1)/ M W for most magnetic refrigerants. Here, we report giant MCE in orthorhombic EuCl 2, where a ferromagnetic ground state with excellent single-ion behavior of Eu 2+ and free spins has been demonstrated by combining ab initio calculations with Brillouin function analysis and magnetic measurements. Consequently, a record-high −Δ S M ∼ 74.6 J·kg –1 ·K –1 (1.8 K) at 5 T was experimentally achieved, approaching 96% of the theoretical limit (77.5 J·kg –1 ·K –1 ). At a lower field of 1 T, EuCl 2 also achieves the highest-ever record of −Δ S M ∼ 36.8 J·kg –1 ·K –1 . Further, direct quasi-adiabatic demagnetization measurements demonstrate that its large −Δ S M allows EuCl 2 to maintain a long holding time at sub-Kelvin temperature (∼346 mK), surpassing all previously reported materials. These superior magnetocaloric performances position EuCl 2 as an attractive cryogenic refrigerant.

Topics & Concepts

Magnetic refrigerationChemistryDemagnetizing fieldAdiabatic processOrthorhombic crystal systemBrillouin and Langevin functionsFerromagnetismAb initioCondensed matter physicsRefrigerantMagnetic fieldThermodynamicsMagnetizationCrystallographyPhysicsCrystal structureGas compressorQuantum mechanicsOrganic chemistryMagnetic and transport properties of perovskites and related materialsPerovskite Materials and ApplicationsThermal Expansion and Ionic Conductivity